Local charge-displacement analysis: Targeting local charge-flows in complex intermolecular interactions.

Area of Science:

• Computational Chemistry
• Quantum Chemistry
• Molecular Interactions

Background:

• Charge-displacement (CD) analysis quantifies charge redistribution in molecular interactions.
• Standard CD analysis provides averaged charge flow profiles for complex interactions.
• Detailed analysis of concurrent charge flows is often needed.

Purpose of the Study:

• To develop a method for detailed, localized analysis of charge redistribution during molecular interactions.
• To introduce Local Charge-Displacement (LCD) analysis by combining CD analysis with Hirshfeld partitioning.
• To apply LCD analysis to systems with complex, multiple charge flows.

Main Methods:

• Combined Charge-Displacement (CD) analysis with Hirshfeld partitioning.
• Developed the Local Charge-Displacement (LCD) analysis scheme.
• Applied LCD analysis to dimethyl sulfide-sulfur dioxide, acetic acid dimer, DNA base pairs, and ammonia-pyridine complex.

Main Results:

• LCD analysis successfully characterized individual charge flows in complex molecular interactions.
• Detailed charge flow profiles were obtained for sulfur-sulfur homochalcogen bonds and hydrogen bonds.
• The method elucidated charge redistribution in various systems including DNA and ambifunctional hydrogen bonds.

Conclusions:

• LCD analysis provides a powerful tool for detailed characterization of localized charge flows.
• This method enhances understanding of complex intermolecular interactions beyond averaged CD analysis.
• LCD analysis is applicable to a wide range of chemical and biological systems.