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

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.

References in corpus (3)

• Quantum embedding theories
• Quantum Embedding Theory for Strongly-correlated States in Materials
• Calculating DMFT forces in ab-initio ultrasoft pseudopotential formalism

Cited by in corpus (3)

• A unified density-matrix functional construction of quantum baths in density matrix embedding theory beyond the mean-field approximation
• Fragment quantum embedding using the Householder transformation: a multi-state extension based on ensembles
• Local Potential Functional Embedding Theory of Molecular Systems: Localized Orbital-Based Embedding from an Exact Density-Functional Perspective