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Cu clusters of nanometer dimensions were created by implantation of Cu ions into pure fused silica substrates at energies of 160 keV. The sizes and size distributions of the Cu clusters were measured by transmission electron microscopy, and were found to be determined by the ion‐beam current during implantation. Optical‐absorption spectra of these materials show the size‐dependent surface plasmon resonance characteristic of noble‐metal clusters. There are also significant size‐dependent effects in both the nonlinear index of refraction and two‐photon absorption coefficients. The distinctive variations in linear and nonlinear optical properties with Cu nanocluster sizes and size distributions affords potentially interesting possibilities for using these materials in nonlinear optical devices.