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Extending Scaled-Interaction Adaptive-Partitioning QM/MM to Covalently Bonded Systems
preprintrevised on 27.05.2020, 09:11 and posted on 28.05.2020, 13:50 by Zenghui Yang
Quantum mechanics/molecular mechanics (QM/MM) is the method of choice for atomistic simulations of large systems that can be partitioned into active and environmental regions. Adaptive-partitioning (AP) methods extend the applicability of QM/MM, allowing active zones to change during the simulation. AP methods achieve continuous potential energy surface (PES) by introducing buffer regions in which atoms have both QM and MM characters. Most of the existing AP-QM/MM methods require multiple QM calculations per time step, which can be expensive for systems with many atoms in buffer regions. Although one can lower the computational cost by grouping atoms into fragments, this may not be possible for all systems, especially for applications in covalent solids. The SISPA method [J. Chem. Theory Comput. 2017, 13, 2342] differs from other AP-QM/MM methods by only requiring one QM calculation per time step, but it has the flaw that the QM charge density and wavefunction near the buffer/MM boundary tend to those of isolated atoms/fragments. Besides, regular QM/MM methods for treating covalent bonds cut by the QM/MM boundary are incompatible with SISPA. Due to these flaws, SISPA in its original form cannot treat covalently bonded systems properly. In this work, I show that a simple modification to the SISPA method improves the treatment of covalently bonded systems. I also study the effect of correcting the charge density in SISPA by developing a density-corrected pre-scaled algorithm. I demonstrate the methods with simple molecules and bulk solids.
Science Challenge Project No. TZ2016003
National Natural Science Foundation of China grant No. 11804314
Email Address of Submitting Authorzenghuiy@gmail.com
InstitutionMicrosystem and Terahertz Research Center, China Academy of Engineering Physics
ORCID For Submitting Author0000-0001-8486-740X
Declaration of Conflict of Interestno conflict of interest
Read the published paper
in Physical Chemistry Chemical Physics