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Charging of materials by incident radiation is affected by both environmental and physical conditions. Modifying a material's physical surface will change its reflection, transmission, and absorption of the incident radiation which are integrally related to the accumulation of charge and energy deposition in the material. General arguments for incident and emitted photons, electrons, and ions are considered. An optical analysis of the effects of surface modification on spacecraft charging parameters on prototypical polyimide Kapton HN and Cu samples is presented. Samples were roughened with abrasive compounds ranging from 0.5 to 10 μm in size, comparable to the range of incident wavelengths. They were also contaminated with thin layers of DC 704 diffusion pump oil. Using a UV/VIS/NIR light source and a diffraction grating spectrometer, measurements were performed on pristine and modified materials. The measured spectra confirmed that surface modifications induce expected changes in optical reflection, transmission, and absorption. The generally increased absorption observed results in increased photon energy deposited in the material, leading to increased charge emission through the photoelectric effect.