Christensen Anders S, Steinmann Casper, Fedorov Dmitri G, Jensen Jan H
Department of Chemistry, University of Copenhagen, Copenhagen, Denmark.
Department of Physics, Chemistry and Pharmacy, University of Southern Denmark, Odense, Denmark.
PLoS One. 2014 Feb 18;9(2):e88800. doi: 10.1371/journal.pone.0088800. eCollection 2014.
The frozen domain effective fragment molecular orbital method is extended to allow for the treatment of a single fragment at the MP2 level of theory. The approach is applied to the conversion of chorismate to prephenate by Chorismate Mutase, where the substrate is treated at the MP2 level of theory while the rest of the system is treated at the RHF level. MP2 geometry optimization is found to lower the barrier by up to 3.5 kcal/mol compared to RHF optimzations and ONIOM energy refinement and leads to a smoother convergence with respect to the basis set for the reaction profile. For double zeta basis sets the increase in CPU time relative to RHF is roughly a factor of two.
冷冻区域有效片段分子轨道方法得到扩展，以允许在MP2理论水平上处理单个片段。该方法应用于分支酸变位酶将分支酸转化为预苯酸的反应，其中底物在MP2理论水平上处理，而系统的其余部分在RHF水平上处理。与RHF优化和ONIOM能量精修相比，发现MP2几何优化可使势垒降低多达3.5 kcal/mol，并使反应剖面图的基组收敛更平滑。对于双ζ基组，相对于RHF，CPU时间增加约两倍。
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