Trajectory Surface Hopping for a Polarizable Embedding QM/MM Formulation.

Area of Science:

• Computational Chemistry
• Quantum Mechanics
• Molecular Dynamics

Background:

• Accurate simulation of nonadiabatic dynamics is crucial for understanding chemical reactions.
• Polarizable embedding QM/MM methods offer a way to model complex systems.
• Existing methods may lack the necessary integration for advanced simulations.

Purpose of the Study:

• To implement and validate a novel trajectory surface-hopping nonadiabatic dynamics method.
• To couple time-dependent density functional theory (TD-DFT) with the polarizable AMOEBA force field.
• To create a robust computational tool for studying photoinduced electron-driven proton transfer reactions.

Main Methods:

• Utilized time-dependent density functional theory (TD-DFT) for quantum mechanical calculations.
• Employed the polarizable AMOEBA force field for molecular mechanics.
• Integrated the Newton-X NS program with Gaussian 16 and Tinker computational chemistry suites.
• Calculated QM/AMOEBA energies and forces for dynamics simulations.

Main Results:

• Successfully implemented trajectory surface-hopping nonadiabatic dynamics within a QM/MM framework.
• Validated the implementation using a photoinduced electron-driven proton transfer reaction.
• Tested the method on systems ranging from small water clusters to large water droplets.

Conclusions:

• The developed QM/MM method provides a powerful tool for simulating nonadiabatic dynamics.
• This approach enables accurate modeling of complex reactions in condensed phases.
• The implementation facilitates the study of electron-driven proton transfer mechanisms.