Constrained nuclear-electronic orbital QM/MM approach for simulating complex systems with quantum nuclear delocalization effects incorporated

被引:3
|
作者
Zhao, Xianyuan
Chen, Zehua
Yang, Yang [1 ]
机构
[1] Univ Wisconsin, Theoret Chem Inst, 1101 Univ Ave, Madison, WI 53706 USA
来源
CHEMICAL PHYSICS REVIEWS | 2024年 / 5卷 / 04期
基金
美国国家科学基金会;
关键词
DENSITY-FUNCTIONAL THEORY; FREE-ENERGY SIMULATIONS; BARRIER HYDROGEN-BONDS; MOLECULAR-DYNAMICS; VIBRATIONAL-SPECTRA; WAVE-FUNCTIONS; FORCE-FIELDS; BASIS-SETS; EFFICIENT; WATER;
D O I
10.1063/5.0226271
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The hybrid quantum mechanics/molecular mechanics (QM/MM) approach, which combines the accuracy of QM methods with the efficiency of MM methods, is widely used in the study of complex systems. However, past QM/MM implementations often neglect or face challenges in addressing nuclear quantum effects, despite their crucial role in many key chemical and biological processes. Recently, our group developed the constrained nuclear-electronic orbital (CNEO) theory, a cost-efficient approach that accurately addresses nuclear quantum effects, especially quantum nuclear delocalization effects. In this work, we integrate CNEO with the QM/MM approach through the electrostatic embedding scheme and apply the resulting CNEO QM/MM to two hydrogen-bonded complexes. We find that both solvation effects and nuclear quantum effects significantly impact hydrogen bond structures and dynamics. Notably, in the glutamic acid-glutamate complex, which mimics a common low barrier hydrogen bond in biological systems, CNEO QM/MM accurately predicts nearly equal proton sharing between the two residues. With an accurate description of both quantum nuclear delocalization effects and environmental effects, CNEO QM/MM is a promising new approach for simulating complex chemical and biological systems.
引用
收藏
页数:11
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