Journal
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
Volume 104, Issue 40, Pages 15705-15710Publisher
NATL ACAD SCIENCES
DOI: 10.1073/pnas.0703279104
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We have implemented the recently demonstrated technique of chirped-pulse upconversion of midinfrared femtosecond pulses into the visible in a visible pump-midinfrared probe experiment for high-resolution, high-sensitivity measurements over a broad spectral range. We have succeeded in time-resolving the CO ligand transfer process from the heme Fe to the neighboring Cu-B atom in the bimetallic active site of mammalian cytochrome c oxidase, which was known to proceed in <1 ps, using the full CO vibrational signature of Fe-CO bond breaking and Cu-B-CO bond formation. Our differential transmission results show a delayed onset of the appearance of the Cu-B-bound species (200 fs), followed by a 450-fs exponential rise. Trajectories calculated by using molecular-dynamics simulations with a Morse potential for the Cu-B-C interaction display a similar behavior. Both experimental and calculated data strongly suggest a ballistic contribution to the transfer process.
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