Combined molecular dynamics and coordinate driving method for automatically searching complicated reaction pathways

Area of Science:

• Computational Chemistry
• Reaction Mechanism Elucidation
• Chemical Dynamics

Background:

• Automated reaction pathway searching is crucial for understanding complex chemical transformations.
• Existing methods often struggle with intricate systems and diverse reaction mechanisms.

Purpose of the Study:

• To update and generalize the combined molecular dynamics and coordinate driving (MD/CD) method.
• To broaden its applicability in automatically searching reaction pathways for complicated reactions.
• To incorporate single electron transfer (SET) processes into reaction pathway exploration.

Main Methods:

• Utilizing the GFN's family of methods for molecular dynamics (MD) simulations to sample conformers.
• Accelerating the coordinate driving (CD) procedure with a pre-screening stage at the GFN2-xTB level.
• Developing an automatic module based on Marcus and Wolynes theories to include SET processes.

Main Results:

• The enhanced MD/CD method successfully explored reaction pathways for three complex reactions.
• Comprehensive reaction networks were obtained with reasonable computational costs.
• Detailed mechanisms elucidated by the method align with experimental observations.

Conclusions:

• The updated MD/CD method provides an efficient and versatile tool for investigating complex reaction mechanisms.
• The inclusion of SET processes expands the scope of reactions that can be studied.
• This advancement facilitates a deeper understanding of chemical reactivity and catalysis.