The excited-state dynamics of molecules embedded in complex
(bio)matrices
is still a challenging goal for quantum chemical models. Hybrid QM/MM
models have proven to be an effective strategy, but an optimal combination
of accuracy and computational cost still has to be found. Here, we
present a method which combines the accuracy of a polarizable embedding
QM/MM approach with the computational efficiency of an excited-state
self-consistent field method. The newly implemented method is applied
to the photoactivation of the blue-light-using flavin (BLUF) domain
of the AppA protein. We show that the proton-coupled electron transfer
(PCET) process suggested for other BLUF proteins is still valid also
for AppA.
We describe the development, implementation, and application of a polarizable QM/MM strategy, based on the AMOEBA polarizable force field, for calculating molecular properties and performing dynamics of molecular systems embedded in complex matrices. We show that polarizable QM/MM is a well‐understood, mature technology that can be deployed using a state‐of‐the‐art implementation that combines efficient numerical methods and linear scaling techniques. Thanks to these numerical advances and to the availability of parameters for a wide manifold of systems in the AMOEBA force field, polarizable QM/AMOEBA can be used for advanced production applications, that range from the prediction of spectroscopies to ground‐ and excited‐state multiscale ab initio molecular dynamics simulations.This article is categorized under:
Electronic Structure Theory > Ab Initio Electronic Structure Methods
Electronic Structure Theory > Combined QM/MM Methods
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