Topological constraints on proton dynamics in water clusters.

Area of Science:

• Physical Chemistry
• Computational Chemistry
• Materials Science

Background:

• Water cluster dynamics are crucial for understanding proton transfer.
• Interconversion of hydrogen-bond (H-bond) configurations is a key process.
• Proton rearrangement networks can be fragmented, posing barriers to dynamics.

Purpose of the Study:

• To investigate the topological connectivity of proton rearrangement networks in water clusters.
• To determine if different H-bond configuration interconversion mechanisms lead to connected or fragmented networks.
• To identify structural features that cause network disintegration.

Main Methods:

• Analytical study using graph theory to assess network connectivity.
• Examination of individual and combined H-bond interconversion mechanisms.
• Numerical analysis of characteristic water clusters.

Main Results:

• Connectivity of proton rearrangement networks is proven for various water clusters.
• Simple H-bond interconversion mechanisms demonstrate significant power in reconfiguring proton networks.
• Specific structural motifs leading to network fragmentation were identified.

Conclusions:

• Proton dynamics in water clusters are facilitated by connected rearrangement networks.
• Graph theory provides a powerful framework for analyzing proton dynamics.
• Findings are relevant for understanding water-based ferroelectrics and proton transport.