Understanding the electronic structure of localized perturbations in crystalline materials often requires accurate as well as affordable correlated wave function-based methods. Examples of such localized perturbations include solid-state defects or the presence of an adsorbate molecule on a solid surface. Solid-state defects are important qubit candidates for quantum information while surface adsorption is a primary step in heterogeneous catalysis. Localized perturbations result in the breakdown of translational symmetry which forces the requirement of large supercells and therefore renders correlated wave function-based methods prohibitively costly. In such cases, quantum embedding provides an attractive balance in the compromise between cost and accuracy such that the “perturbations” (here the defects/region of adsorption) are treated with a high-level method whereas the rest of the system is treated with a mean field method. Here, we discuss our recent developments using the density matrix embedding theory (DMET) algorithm to study electronic excitations in solid-state defects and binding energies of gas molecules on solid-state surfaces. We find good agreement between DMET using correlated wave function-based solvers and the non-embedded approaches. We further show that DMET can be used to find the excitation energies of large supercells where the use of conventional non-embedded methods become intractable.

Local Excitations in Spin Defects and Surface Binding using Density Matrix Embedding Theory

Fall 2022 abstracts, posters, and presentations will launch in mid-September.

ACS Fall 2022

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.