Coherent Vibrational Climbing in Carboxyhemoglobin

We demonstrate vibrational climbing in the CO stretch of carboxy-hemoglobin 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,...

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Published inProceedings of the National Academy of Sciences - PNAS Vol. 101; no. 36; pp. 13216 - 13220
Main Authors Ventalon, Cathie, Fraser, James M., Vos, Marten H., Alexandrou, Antigoni, Martin, Jean-Louis, Joffre, Manuel, Frauenfelder, Hans
Format Journal Article
LanguageEnglish
Published United States National Academy of Sciences 07.09.2004
National Acad Sciences
Subjects
Absorption spectra
Biological Sciences
Biophysics
Carboxyhemoglobin - chemistry
Chirp
Curves
Delay lines
Efficiency
Ground state
Molecules
Population growth
Pumps
Signals
Spectrum Analysis
Vibration
Vibration analysis
Vibrational states
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Summary:We demonstrate vibrational climbing in the CO stretch of carboxy-hemoglobin 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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PMCID: PMC516550
Edited by Hans Frauenfelder, Los Alamos National Laboratory, Los Alamos, NM, and approved June 22, 2004
To whom correspondence should be addressed. E-mail: manuel.joffre@polytechnique.fr.
This paper was submitted directly (Track II) to the PNAS office.
ISSN:0027-8424
1091-6490
DOI:10.1073/pnas.0401844101