Journal of Chemical Theory and Computation, volume 11, issue 8, pages 3878-3894
Role of the Molecular Environment in Flavoprotein Color and Redox Tuning: QM Cluster versus QM/MM Modeling
3
Chemistry Department, Overman
Hall, Bowling Green State University, Bowling
Green, Ohio 67200, United States
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Publication type: Journal Article
Publication date: 2015-07-20
Quartile SCImago
Q1
Quartile WOS
Q1
Impact factor: 5.5
ISSN: 15499618, 15499626
Physical and Theoretical Chemistry
Computer Science Applications
Abstract
We investigate the origin of the excitation energy shifts induced by the apoprotein in the active site of the bacterial photoreceptor BLUF (Blue Light sensor Using Flavin adenine dinucleotide). In order to compute the vertical excitation energies of three low-lying electronic states, including two π-π* states of flavin (S1 and S2) and a π-π* tyrosine-flavin electron-transfer state (ET), with respect to the energy of the closed-shell ground state (S0), we prepared alternative quantum mechanical (QM) cluster and quantum mechanics/molecular mechanics (QM/MM) models. We found that the excitation energies computed with both types of models correlate with the magnitude of the charge transfer character of the excitation. Accordingly, we conclude that the small charge transfer character of the light absorbing S0-S1 transition and the substantial charge transfer character of the nonabsorbing but redox active S0-ET transition explain the small color changes but substantial redox tuning in BLUF and also in other flavoproteins. Further analysis showed that redox tuning is governed by the electrostatic interaction in the QM/MM model and transfer of charge between the active site and its environment in the QM cluster. Moreover, the wave function polarization of the QM subsystem by the MM subsystem influences the magnitude of the charge transfer, resulting in the QM/MM and QM excitation energies that are not entirely consistent.
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Udvarhelyi A. et al. Role of the Molecular Environment in Flavoprotein Color and Redox Tuning: QM Cluster versus QM/MM Modeling // Journal of Chemical Theory and Computation. 2015. Vol. 11. No. 8. pp. 3878-3894.
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Udvarhelyi A., Olivucci M., Domratcheva T. Role of the Molecular Environment in Flavoprotein Color and Redox Tuning: QM Cluster versus QM/MM Modeling // Journal of Chemical Theory and Computation. 2015. Vol. 11. No. 8. pp. 3878-3894.
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TY - JOUR
DO - 10.1021/acs.jctc.5b00197
UR - https://doi.org/10.1021%2Facs.jctc.5b00197
TI - Role of the Molecular Environment in Flavoprotein Color and Redox Tuning: QM Cluster versus QM/MM Modeling
T2 - Journal of Chemical Theory and Computation
AU - Udvarhelyi, Anikó
AU - Olivucci, Massimo
AU - Domratcheva, Tatiana
PY - 2015
DA - 2015/07/20 00:00:00
PB - American Chemical Society (ACS)
SP - 3878-3894
IS - 8
VL - 11
SN - 1549-9618
SN - 1549-9626
ER -
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@article{2015_Udvarhelyi,
author = {Anikó Udvarhelyi and Massimo Olivucci and Tatiana Domratcheva},
title = {Role of the Molecular Environment in Flavoprotein Color and Redox Tuning: QM Cluster versus QM/MM Modeling},
journal = {Journal of Chemical Theory and Computation},
year = {2015},
volume = {11},
publisher = {American Chemical Society (ACS)},
month = {jul},
url = {https://doi.org/10.1021%2Facs.jctc.5b00197},
number = {8},
pages = {3878--3894},
doi = {10.1021/acs.jctc.5b00197}
}
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MLA
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Udvarhelyi, Anikó, et al. “Role of the Molecular Environment in Flavoprotein Color and Redox Tuning: QM Cluster versus QM/MM Modeling.” Journal of Chemical Theory and Computation, vol. 11, no. 8, Jul. 2015, pp. 3878-3894. https://doi.org/10.1021%2Facs.jctc.5b00197.
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