Embedded Localized Molecular-Orbital Representations for Periodic Wave Functions

To more straightforwardly provide local chemical-bondingreasoningin crystalline matter, we introduce a new approach to generate a real-spaceanalogue of periodic electronic structures using "exact"top-down frozen-density embedding calculations. Based on the obtainedreal-space electronic structure, we then construct localized molecularorbitals and evidence that our technique compares favorably againstthe commonly used Wannier method, both in terms of numerical efficiencyand details of chemical bonding. The new method has been implementedinto the LOBSTER software package and designed as a black-box approach,digesting any periodic electronic structure from the currently supportedcodes, i.e., VASP, Quantum ESPRESSO, and ABINIT.