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Diamond materials are central to an increasing range of advancedtechnological demonstrations, from high power electronics, to nano-scalequantum bio-imaging with unprecedented sensitivity. However, the fullexploitation of diamond for these applications is often limited by theuncontrolled nature of the diamond material surface, which suffers fromFermi-level pinning and hosts a significant density of electro-magnetic noisesources. These issues occur despite the oxide-free and air-stable nature of thediamond crystal surface, which should be an ideal candidate forfunctionalization and chemical-engineering. In this work we reveal a family ofpreviously unidentified and near-ubiquitous primal surface defects which weassign to differently reconstructed surface vacancies. The density of thesedefects is quantified with X-ray absorption spectroscopy, their energystructures are elucidated by ab initio calculations, and their effect onnear-surface quantum probes is measured directly. Subsequent ab-initiocalculation of band-bending from these defects suggest they are the source ofFermi-level pinning at most diamond surfaces. Finally, an investigation isconducted on a broad range of post-growth surface treatments and concludes thatnone of them can reproducibly reduce this defect density below theFermi-pinning threshold, making this defect a prime candidate as the source fordecoherence-limiting noise in near-surface quantum probes.

Evidence for Primal sp2 Defects at the Diamond Surface: Candidates for Electron Trapping and Noise Sources