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Issue 39, 2011
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Ultrafast transient mid IR to visible spectroscopy of fully reduced flavins

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Abstract

The light sensing apparatus of many organisms includes a flavoprotein. In any spectroscopic analysis of the photocycle of flavoproteins a detailed knowledge of the spectroscopy and excited state dynamics of potential intermediates is required. Here we correlate transient vibrational and electronic spectra of the two fully reduced forms of flavin adenine dinucleotide (FAD): FADH and FADH2. Ground and excited state frequencies of the characteristic carbonyl modes are observed and assigned with the aid of DFT calculations. Excited state decay and ground state recovery dynamics of the two states are reported. Excited state decay occurs on the picosecond timescale, in agreement with the low fluorescence yield, and is markedly non single exponential in FADH. Further, an unusual ‘inverse’ isotope effect is observed in the decay time of FADH, suggesting the involvement in the radiationless relaxation coordinate of an NH or hydrogen bond mode that strengthens in the excited electronic state. Ground state recovery also occurs on the picosecond time scale, consistent with radiationless decay by internal conversion, but is slower than the excited state decay.

Graphical abstract: Ultrafast transient mid IR to visible spectroscopy of fully reduced flavins

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Publication details

The article was received on 27 Jun 2011, accepted on 11 Aug 2011 and first published on 01 Sep 2011


Article type: Paper
DOI: 10.1039/C1CP22097G
Citation: Phys. Chem. Chem. Phys., 2011,13, 17642-17648
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    Ultrafast transient mid IR to visible spectroscopy of fully reduced flavins

    R. Zhao, A. Lukacs, A. Haigney, R. Brust, G. M. Greetham, M. Towrie, P. J. Tonge and S. R. Meech, Phys. Chem. Chem. Phys., 2011, 13, 17642
    DOI: 10.1039/C1CP22097G

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