The effect of local substrate motion on quantum hydrogen transfer in soybean lipoxygenase-1 modeled with QTES-DFTB dynamics

James W. Mazzuca; Sophya Garashchuk; Jacek Jakowski

doi:10.1016/j.cplett.2014.08.006

The effect of local substrate motion on quantum hydrogen transfer in soybean lipoxygenase-1 modeled with QTES-DFTB dynamics

James W. Mazzuca, Sophya Garashchuk, Jacek Jakowski

Research output: Contribution to journal › Article › peer-review

7 Scopus citations

Abstract

The motion of local substrate nuclei is incorporated into the quantum hydrogen transfer reaction which occurs in the active site of soybean lipoxygenase-1, modeled within a quantum trajectory (QT) framework. Interactions within the active site are obtained from on-the-fly electronic structure (ES) calculations at the density-functional tight-binding (DFTB) level. By selectively constraining substrate nuclei, changes in the rate constants and kinetic isotope effect are computed over a 100 K temperature range. Substrate motion, occurring on the time-scale of the hydrogen transfer, enhances both the rate constants and isotope effect, but does not change trends captured in a constrained substrate environment.

Original language	English
Pages (from-to)	104-109
Number of pages	6
Journal	Chemical Physics Letters
Volume	613
DOIs	https://doi.org/10.1016/j.cplett.2014.08.006
State	Published - Oct 3 2014
Externally published	Yes

Funding

This material is based upon work partially supported by the National Science Foundation under Grants No. CHE-1056188 and CHE-1048629 , as well as EPSCoR GEAR:CI (J.M. and S.G.). Additional support was provided by the National Science Foundation Grant No. APRA-NSF-EPS-0919436 (J.J.). The XSEDE allocation TG-DMR110037 for time on Kraken at the National Institute for Computational Sciences is also acknowledged.

Funders	Funder number
EPSCoR GEAR	APRA-NSF-EPS-0919436
National Science Foundation	CHE-1056188, CHE-1048629, 1048629, 1056188

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10.1016/j.cplett.2014.08.006

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abstract = "The motion of local substrate nuclei is incorporated into the quantum hydrogen transfer reaction which occurs in the active site of soybean lipoxygenase-1, modeled within a quantum trajectory (QT) framework. Interactions within the active site are obtained from on-the-fly electronic structure (ES) calculations at the density-functional tight-binding (DFTB) level. By selectively constraining substrate nuclei, changes in the rate constants and kinetic isotope effect are computed over a 100 K temperature range. Substrate motion, occurring on the time-scale of the hydrogen transfer, enhances both the rate constants and isotope effect, but does not change trends captured in a constrained substrate environment.",

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AU - Jakowski, Jacek

PY - 2014/10/3

Y1 - 2014/10/3

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AB - The motion of local substrate nuclei is incorporated into the quantum hydrogen transfer reaction which occurs in the active site of soybean lipoxygenase-1, modeled within a quantum trajectory (QT) framework. Interactions within the active site are obtained from on-the-fly electronic structure (ES) calculations at the density-functional tight-binding (DFTB) level. By selectively constraining substrate nuclei, changes in the rate constants and kinetic isotope effect are computed over a 100 K temperature range. Substrate motion, occurring on the time-scale of the hydrogen transfer, enhances both the rate constants and isotope effect, but does not change trends captured in a constrained substrate environment.

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VL - 613

SP - 104

EP - 109

JO - Chemical Physics Letters

JF - Chemical Physics Letters

ER -

The effect of local substrate motion on quantum hydrogen transfer in soybean lipoxygenase-1 modeled with QTES-DFTB dynamics

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