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The authors report here on a new technique, combining the atomic precision of molecular beam epitaxy and atomic layer deposition, to fabricate back illuminated silicon CCD detectors that demonstrate world record detector quantum efficiency (>50%) in the near and far ultraviolet (155–300 nm). This report describes in detail the unique surface engineering approaches used and demonstrates the robustness of detector performance that is obtained by achieving atomic level precision at key steps in the fabrication process. The characterization, materials, and devices produced in this effort will be presented along with comparison to other approaches.