An efficient and flexible approach for local distortion: distortion distribution analysis enabled by fragmentation

Area of Science:

• Chemical Physics
• Computational Chemistry
• Molecular Dynamics

Background:

• Distortion significantly influences molecular structures, properties, reactivity, and selectivity in chemical and biological systems.
• The distortion/interaction or activation-strain model explains activation energies, but atomic-scale local distortion energy decomposition is unclear.
• Understanding local distortion is crucial for deeper insights into reaction processes and improved reaction design.

Purpose of the Study:

• To develop an efficient, general, and flexible fragmentation-based approach for evaluating local distortion energies.
• To provide a method applicable to various chemical and biological molecules, obtainable both computationally and experimentally.
• To offer deeper insights into reaction mechanisms and dynamics.

Main Methods:

• A novel fragmentation-based approach was developed to calculate local distortion energies.
• The method is applicable to diverse molecular structures, including those from molecular dynamics simulations or minimum energy paths.
• Distortion analysis can be performed using various computational chemistry methods.

Main Results:

• The approach enables visualization of relative distortion distributions within molecules, creating a 'distortion map'.
• It successfully identifies key distorted molecular fragments.
• The method provides indices of local distortion energy.

Conclusions:

• The developed approach offers a clear method for evaluating local distortion energies at the atomic scale.
• It enhances the understanding of structures, reaction mechanisms, and dynamics in chemical and biological systems.
• Local distortion energy indices can serve as valuable descriptors for multi-linear regression and machine learning modeling.