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Proton Transfer in Bulk Water using the Full Adaptive QM/MM Method: Integration of Solute- and Solvent-Adaptive Approaches

preprint
revised on 31.12.2020, 01:14 and posted on 31.12.2020, 12:11 by Hiroshi C. Watanabe, Masayuki Yamada, Yohichi Suzuki
The quantum mechanical/molecular mechanical (QM/MM) method is a hybrid molecular simulation technique that increases the accessibility of local electronic structures of large systems.
The technique combines the benefit of accuracy found in the QM method and that of cost efficiency found in the MM method.
However, it is difficult to directly apply the QM/MM method to the dynamics of solution systems, particularly for proton transfer.
As explained in the Grotthuss mechanism, proton transfer is a structural interconversion between hydronium ions and solvent water molecules.
Hence, when the QM/MM method is applied, an adaptive treatment, namely on-the-fly revisions on molecular definitions, is required for both the solute and solvent.
Although several solvent-adaptive methods have been proposed, a full adaptive framework, which is an approach that also considers adaptation for solutes, remains untapped. In this paper, we propose a new numerical expression for the coordinates of the excess proton and its control algorithm.
Furthermore, we confirm that this method can stably and accurately simulate proton transfer dynamics in bulk water.

Funding

JSPS Grant Number 20K03885

JSPS Grant Number 20H05518

JST PRESTO Grant number JPMJPR17GC.

the MEXT Quantum Leap Flagship Program Grant Number JPMXS0118067285.

History

Email Address of Submitting Author

hcwatanabe@keio.jp

Institution

Keio University

Country

Japan

ORCID For Submitting Author

0000-0003-4379-8633

Declaration of Conflict of Interest

No conflict of interest

Version Notes

In the previous versions, there were bugs in the program for the calculation in derivative of the QM center. Hence, we modified it and recalculated all relevant data. According to it, we also rewrite discussions.

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