Electron Density Transport During Chemical Reactions

Area of Science:

• Computational Chemistry
• Theoretical Chemistry
• Chemical Physics

Background:

• Statistical methods are crucial for analyzing electronic structure changes during chemical reactions and molecular excitations.
• High-throughput studies require computationally efficient methods with minimal data preprocessing.

Purpose of the Study:

• To investigate optimal transport (OT) as a method for characterizing electronic structure changes.
• To apply OT to electron densities along a reaction coordinate to understand noncore electron density evolution.

Main Methods:

• Optimal transport (OT) was used to compare probability distributions of electron densities.
• The method was applied to Bergman cyclization and proton transfer in a water cluster.
• Analysis involved partitioning the transport plan to track electron density evolution.

Main Results:

• OT provided chemically intuitive insights into Bergman cyclization, complementing the electron localization function.
• For proton transfer, OT clearly identified individual transfer events in ab initio molecular dynamics simulations.
• The approach demonstrated effectiveness in analyzing electron density dynamics.

Conclusions:

• Optimal transport is a promising new framework for studying chemical reactivity.
• The method offers computational efficiency and requires minimal data preprocessing.
• OT provides valuable insights into the evolution of electron density during chemical processes.