Low-frequency dynamics of Caldariomyces fumago chloroperoxidase probed by femtosecond coherence spectroscopy.

Biochemistry
Flaviu GruiaPaul M Champion

Abstract

Ultrafast laser spectroscopy techniques are used to measure the low-frequency vibrational coherence spectra and nitric oxide rebinding kinetics of Caldariomyces fumago chloroperoxidase (CPO). Comparisons of the CPO coherence spectra with those of other heme species are made to gauge the protein-specific nature of the low-frequency spectra. The coherence spectrum of native CPO is dominated by a mode that appears near 32-33 cm(-1) at all excitation wavelengths, with a phase that is consistent with a ground-state Raman-excited vibrational wavepacket. On the basis of a normal coordinate structural decomposition (NSD) analysis, we assign this feature to the thiolate-bound heme doming mode. Spectral resolution of the probe pulse ("detuned" detection) reveals a mode at 349 cm(-1), which has been previously assigned using Raman spectroscopy to the Fe-S stretching mode of native CPO. The ferrous species displays a larger degree of spectral inhomogeneity than the ferric species, as reflected by multiple shoulders in the optical absorption spectra. The inhomogeneities are revealed by changes in the coherence spectra at different excitation wavelengths. The appearance of a mode close to 220 cm(-1) in the coherence spectrum of reduced CPO e...Continue Reading

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Citations

Oct 4, 2011·Journal of the American Chemical Society·Venugopal KarunakaranPaul M Champion
Jul 4, 2008·Journal of the American Chemical Society·Minoru KuboPaul M Champion
Mar 12, 2011·The Journal of Physical Chemistry. B·Venugopal KarunakaranPaul M Champion
Feb 17, 2010·The Journal of Physical Chemistry. B·Venugopal KarunakaranPaul M Champion
Jul 19, 2013·The Journal of Physical Chemistry. B·Yuhan SunPaul M Champion
Dec 21, 2010·Archives of Biochemistry and Biophysics·Abhinav LuthraStephen G Sligar
Mar 31, 2015·Biophysical Chemistry·Ines DelfinoMaria Lepore
Aug 16, 2016·International Journal of Molecular Sciences·Alexander N Morozov, David C Chatfield

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