Large-Scale Ab Initio Molecular Dynamics for Assessing Stabilities of Near-Surface NV Centers

Near-surface nitrogen vacancy (NV) centers are promising candidate materials for quantum sensors, but their properties have not been examined as thoroughly compared to their bulk counterparts. To shed mechanistic insight into their electronic properties and stabilities, we present the first ab initio molecular dynamics study and quantum mechanical analysis of these near-surface NV center configurations. Our ab initio calculations predict that NV centers near the 111 surface are more energetically stable than defects located deeper in the diamond structure. Moreover, our ab initio molecular dynamics calculations indicate that these near-surface NV centers are stable at high temperatures as high as 1000 C. Our results are complemented by Crystal Orbital Hamilton Population (COHP) analyses and calculations of other low-lying electronic-excited states to quantify the electronic properties and stabilities of these structures that could form the materials used in next-generation quantum sensors.