Accurate and Efficient Spin-Spin Zero-Field Splitting Calculations for Extended Periodic Systems

Abstract

Spin-spin zero-field splitting (ZFS) is a sensitive spectroscopic signature accessable by electron paramagnetic resonance. It is the key fingerprint used for the identification of high-spin defect centers in semiconducting host materials and for the characterization of their electronic structure. In recent years, much progress has been made in developing an efficient first-principles methodology for ZFS calculations that help in the interpretation of experimental data. Here we address the negatively charged nitrogen-vacancy center (NV −) in diamond. It is used as a test system to explore the accuracy and efficiency of spin-spin zero-field splitting calculations on massively parallel computing systems.