Multi-site Reaction Dynamics Through Multi-fragment Density Matrix Embedding

TL;DR

This paper develops a gradient theory for multi-fragment density matrix embedding, enabling efficient modeling of complex multi-site chemical reactions at the correlated electron level, demonstrated through validation and a water cluster simulation.

Contribution

It introduces the gradient theory for multi-fragment density matrix embedding, advancing the computational modeling of multi-site reactions with correlated electrons.

Findings

Validated on model systems and chemical reactions.

Successfully applied to simulate proton transport in water clusters.

Provides a minimal framework for multi-site reaction dynamics.

Abstract

The practical description of disordered chemical reactions, where reactions involve multiple species at multiple sites, is presently challenge using correlated electronic structure methods. Here we describe the gradient theory of multi-fragment density matrix embedding theory, which potentially provides a minimal computational framework to model such processes at the correlated electron level. We present the derivation and implementation of the gradient theory, its validation on model systems and chemical reactions using density matrix embedding, and its application to a molecular dynamics simulation of proton transport in a small water cluster, a simple example of multi-site reaction dynamics.