COMMUNICATION
(1 of 8)Diamond materials are central to an increasing range of advanced technological demonstrations, from high power electronics to nanoscale quantum bioimaging with unprecedented sensitivity. [1] However, the full exploitation of diamond for these applications is often limited by the uncontrolled nature of the diamond material surface, which suffers from Fermi-level pinning and hosts a significant density of electromagnetic noise sources. [2] These issues occur despite the oxide-free and air-stable nature of the diamond crystal surface, which should be an ideal candidate for functionalization and chemical engineering. In this work, a family of previously unidentified and near-ubiquitous primal surface defects, which are assigned to differently reconstructed surface vacancies, is revealed. The density of these defects is quantified with X-ray absorption spectroscopy, their energy structures are elucidated by ab initio calculations, and their effect on near-surface quantum Many advanced applications of diamond materials are now being limited by unknown surface defects, including in the fields of high power/ frequency electronics and quantum computing and quantum sensing. Of acute interest to diamond researchers worldwide is the loss of quantum coherence in near-surface nitrogen-vacancy (NV) centers and the generation of associated magnetic noise at the diamond surface. Here for the first time is presented the observation of a family of primal diamond surface defects, which is suggested as the leading cause of band-bending and Fermi-pinning phenomena in diamond devices. A combination of density functional theory and synchrotron-based X-ray absorption spectroscopy is used to show that these defects introduce low-lying electronic trap states. The effect of these states is modeled on band-bending into the diamond bulk and it is shown that the properties of the important NV defect centers are affected by these defects. Due to the paramount importance of near-surface NV center properties in a growing number of fields, the density of these defects is further quantified at the surface of a variety of differently-treated device surfaces, consistent with best-practice processing techniques in the literature. The identification and characterization of these defects has wide-ranging implications for diamond devices across many fields.