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Quantum chemical calculations of tryptophan→heme electron and excitation energy transfer rates in myoglobin

Suess, Christian J.; Hirst, Jonathan D.; Besley, Nicholas A.

Authors

Christian J. Suess

Nicholas A. Besley



Abstract

The development of optical multidimensional spectroscopic techniques has opened up new possibilities for the study of biological processes. Recently, ultrafast two- dimensional ultraviolet spectroscopy experiments have determined the rates of tryptophan→heme electron transfer and excitation energy transfer for the two tryptophan residues in myoglobin [Consani et al., Science, 2013, 339, 1586]. Here we show that accurate prediction of these rates can be achieved using Marcus theory in conjunction with time-dependent density functional theory (TDDFT). Key intermediate residues between the donor and acceptor are identified, and in particular the residues Val68 and Ile75 play a critical role in calculations of the electron coupling matrix elements. Our calculations demonstrate how small changes in structure can have a large effect on the rates, and show that the different rates of electron transfer are dictated by the distance between the heme and tryptophan residues, while for excitation energy transfer the orientation of the tryptophan residues relative to the heme is important.

Citation

Suess, C. J., Hirst, J. D., & Besley, N. A. (2017). Quantum chemical calculations of tryptophan→heme electron and excitation energy transfer rates in myoglobin. Journal of Computational Chemistry, 38(17), 1495-1502. https://doi.org/10.1002/jcc.24793

Journal Article Type Article
Acceptance Date Mar 3, 2017
Online Publication Date Apr 1, 2017
Publication Date Jun 30, 2017
Deposit Date Mar 23, 2017
Publicly Available Date Apr 1, 2017
Journal Journal of Computational Chemistry
Print ISSN 0192-8651
Electronic ISSN 1096-987X
Publisher Wiley
Peer Reviewed Peer Reviewed
Volume 38
Issue 17
Pages 1495-1502
DOI https://doi.org/10.1002/jcc.24793
Keywords Myoglobin, Electron transfer, Excitation energy transfer, TDDFT
Public URL http://eprints.nottingham.ac.uk/id/eprint/41506
Publisher URL http://onlinelibrary.wiley.com/doi/10.1002/jcc.24793/abstract
Copyright Statement Copyright information regarding this work can be found at the following address: http://creativecommons.org/licenses/by/4.0

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Copyright Statement
Copyright information regarding this work can be found at the following address: http://creativecommons.org/licenses/by/4.0





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