We investigate the microscopic origin of size-dependent magnetization suppression in Ni nanocrystals using photoemission measurements with variable probing depth. While the interior retains bulklike electronic states, the near-surface region exhibits enhanced electronic correlation, leading to conduction-electron localization and the emergence of a magnetic dead layer. This intrinsic modification proves the validity of the dead-layer model quantitatively describing the size dependence of the saturation magnetization. These findings establish a direct link between surface electronic correlation and magnetism at reduced dimensions.

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• Electronic structure
• Magnetic nanoparticles
• Chemical synthesis
• Hard x-ray photoelectron spectroscopy
• Magnetization measurements
• Photoemission spectroscopy