Ghost Embedding Bridging Chemistry and One-Body Theories

TL;DR

This paper introduces a rigorous framework and computational method to connect strongly correlated many-body systems with an effective one-body quasiparticle description, enhancing understanding and prediction of complex chemical behaviors.

Contribution

It presents a novel theoretical and computational approach to bridge strongly correlated systems with effective one-body models using the ghost Gutzwiller Ansatz.

Findings

Successfully applied to Woodward-Hoffmann rules

Reformulated reaction scenarios demonstrating the framework's effectiveness

Provides a new tool for analyzing strongly correlated chemical systems

Abstract

Phenomenological rules play a central role in the design of chemical reactions and materials with targeted properties. Typically, these are formulated heuristically in terms of non-interacting orbitals and bands, yet show remarkable accuracy in predicting the complex behavior of intrinsically interacting many-body systems. While their non-interacting formulation makes them easy to interpret, it potentially hinders the development of new rules for systems governed by strong correlation, such as transition metal-based materials. In this work, we present a rigorous framework that allows bridging between fully interacting, even strongly correlated, systems and an effective one-body picture in terms of quasiparticles. Further, we present a computational strategy to efficiently and accurately access the main components of such a description: the embedding approximation of the ghost Gutzwiller Ansatz. We illustrate the capabilities of this quasiparticle formulation on the Woodward-Hoffmann rules, and apply their reformulated version to toy ``reactions'' which exemplify the main scenarios covered by them.